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“Square‐within‐a‐square”: The first Cr–Dy single‐molecule magnet (SMM) with an energy barrier to spin reorientation of 15 K is presented. The anisotropy in this octanuclear compound arises from the orientations of the four DyIII centers (dark blue), which, in conjunction with the contributions from the CrIII centers (green), leads to the SMM behavior.
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